Composites: Part B 43 (2012) 3549–3562

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Composites: Part B
journal homepage: www.elsevier.com/locate/compositesb

Critical factors on manufacturing processes of natural fibre composites

Mei-po Ho a, Hao Wang a, Joong-Hee Lee b, Chun-kit Ho c, Kin-tak Lau a,d,⇑, Jinsong Leng e, David Hui f
a
Centre of Excellence in Engineered Fibre Composites, Faculty of Engineering and Surveying, University of Southern Queensland, Toowoomba, Queensland, Australia
b
Department of BIN Fusion Technology, Chonbuk National University, Jeonju, Republic of Korea
c
Department of Physics, The University of Science and Technology, Hong Kong, SAR, China
d
Department of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon, Hong Kong, SAR, China
e
Smart Materials and Structures Laboratory, Harbin Institute of Technology, China
f
Department of Mechanical Engineering, University of New Orleans, New Orleans, LA 70148, USA

a r t i c l e i n f o a b s t r a c t

Article history: Elevated environmental awareness of the general public in reducing carbon footprints and the use non-
Received 21 September 2011 naturally decomposed solid wastes has resulted in an increasing use of natural materials, biodegradable
Accepted 3 October 2011 and recyclable polymers and their composites for a wide range of engineering applications. The proper-
Available online 17 October 2011
ties of natural fibre reinforced polymer composites are generally governed by the pre-treated process of
fibre and the manufacturing process of the composites. These properties can be tailored for various types
Keywords: of applications by properly selecting suitable fibres, matrices, additives and production methods. Besides,
E: Manufacturing process
due to the complexity of fibre structures, different mechanical performances of the composites are
A: Natural fibre
obtained even with the use of the same fibre types with different matrices. Some critical issues like poor
wettability, poor bonding and degradation at the fibre/matrix interface (a hydrophilic and hydrophobic
effect) and damage of the fibre during the manufacturing process are the main causes of the reduction
of the composites’ strength. In this paper, different manufacturing processes and their suitability for
natural fibre composites, based on the materials, mechanical and thermal properties of the fibres and
matrices are discussed in detail.
Crown Copyright Ó 2011 Published by Elsevier Ltd. All rights reserved.

1. Introduction ‘‘biocomposites’’) with controllable mechanical properties and bio-

Petroleum is a fossil fuel which is estimated to last for only an-
other 50–60 years at the current rate of consumption [1]. Elevated
environmental consciousness in the general public and preserva-
tion of non-renewable petroleum-based materials especially for
petroleum-based plastics have resulted in an extensive use of nat-
ural fibre reinforced polymer composites for commercial and med-
ical applications. Excessive use of petroleum-based plastics causes
to a serious depletion of landfill capacities. Besides, the severe gov-
ernment’s plastic waste control legislations and the growing inter-
est among the customers in sustainable and environmentally
friendly products drive the retailers and manufacturers trending
towards their investment on the development of sustainable mate-
rials with acceptable cost, to alleviate an impact from global warm-
ing (including the reduction of carbon footprints). Therefore, the
public awareness of increased un-decomposable solid wastes and
their impact to the environment has awakened a new interest in
the area of developing fully biodegradable polymers (also called
⇑ Corresponding author at: Centre of Excellence in Engineered Fibre Composites,
Faculty of Engineering and Surveying, University of Southern Queensland,
Toowoomba, Queensland, Australia.
E-mail addresses: mmktlau@polyu.edu.hk, Kin-tak.Lau@usq.edu.au (K.-t. Lau).
degradation rate.
Recently, biodegradable materials have continued attracting
much attention worldwide. Within the period of 2005 and 2009,
the global market on the demand of biodegradable polymers was
double in size. Among all countries in the World in 2009, Europe
had the largest growth in the range of 5–10% on the use of biode-
gradable polymers as compared with 2008. The total consumption
of biodegradable polymers is forecasted to grow at an average an-
nual rate of nearly 13% from 2009 to 2014 in North America, Europe
and Asia, which are accounted as the major global markets for
materials’ consumption [2]. However, high price and limited prop-
erties of the fully degradable polymer hinder the diversity of the
usage. Therefore, in order to tackle on these problems and retard
the exhaustion of natural resources, different projects along the line
of developing biodegradable composites have emerged recently
and it is general believed that these are one of most key materials
in all industries in coming centuries. In aircraft and automotive
engineering industries, some new projects have been created on
the use of natural fibre (hemp, flax) reinforced biodegradable and
fire-proof polymer composites. Natural fibre biodegradable poly-
mer composites are generally defined as a type of materials which
are generally composed of natural fibre and biodegradable polymer,
as a matrix. The properties of these composites can be tailored for

1359-8368/$ - see front matter Crown Copyright Ó 2011 Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.compositesb.2011.10.001
3550 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
various types of applications by a proper selection of fibres, matrix,
additives and manufacturing process. The pre-treatment process of
fibre plays a key role it controls the overall interfacial bonding prop-
erties and thus, successful stress transfer of resultant composites.
Normally, natural fibre polymer composites are fabricated by
using traditional manufacturing techniques which are designed
for conventional fibre reinforced polymer composites and thermo-
plastics. These techniques include resin transfer moulding (RTM),
vacuum infusion, compression moulding, direct extrusion, com-
pounding and injection moulding. Nevertheless, such techniques
have been well developed and accumulated experience has proofed
their successability for producing composites with controllable
quality. However, their suitability for natural fibre reinforced poly-
mer composites is still unsure due to the materials, geometrical,
mechanical, thermal and structural properties of the natural fibres
and biodegradable polymers are somehow, different with synthetic
fibres and petroleum-based plastics, respectively. For example,
chemical treatments on the fibre surface are normally required to
compensate its incompatible bonding effect at the interface be-
tween the hydrophilic fibre and hydrophobic matrix. Other techni-
cal problems such as the uniformity of fibre distributed inside the
composites, thermal degradations and weathering effect of fibre
and matrix, water absorption of both fibre and matrix, wettability
of resin impregnated into spaces between fibrils and breakage of
fibres during mechanical stirring/mixing stages during the manu-
facturing processes also limit the use of natural fibres and biode-
gradable polymers for new composite development. Recently,
seeking for technologies for developing fireproof natural fibre rein-
forced polymer composites is also one of key topics worldwide to
apply them for aircraft interior components. Therefore, the resul-
tant properties of composites in relation to the selections of right
materials, pre-processing methods and manufacturing process are
inextricably intertwined. In this article, different types of natural fi-
bres and biodegradable polymers, their specific pre-processing
techniques and fabrication methods are introduced and discussed
in detail.
2. Materials selections
2.1. Natural fibres
Natural fibre is a type of renewable sources and a new gener-
ation of reinforcements and supplements for polymer based
materials. Briefly grouping different categories of natural fibres,
they can be divided based on their origin, derivations of plant,
animal and mineral types which are detailedly shown in Fig. 1,
[3–6]. These sustainable and eco-efficient fibres have been ap-
plied as substitutions for glass fibre and other synthetic polymer
fibres for diverse engineering applications. Their remarkable
advantages compared with those conventional inorganic man-
made fillers enhance their commercial and research potentials.
Natural fibres normally are abundantly-renewable resource so
that their cost is relatively low as compared with other synthetic
fibres. With the consideration of environmental consciousness,
natural fibres are biodegradable so as they can alleviate the prob-
lem of massive solid wastes produced and relief the pressure of
landfills if they are used for replacing other non-degradable mate-
rials for product development. Besides, according to their inherent
properties, natural fibres are flexible for processing due to their
less susceptible to machine tool damage and health hazards dur-
ing the manufacturing and etc. Moreover, natural fibres possess
many advantageous characteristics such as desirable fibre aspect
ratio, low density and relatively high tensile and flexural moduli
[7]. Table 1 summarizes the mechanical properties of natural
and man-made fibres.
2.2. Plant-based fibres
By grinding the bark, the cell walls of most plant-based fibres
can be viewed in Fig. 2a. The schematic representation of the cell
wall of a natural plant is shown in Fig. 2b and this structure is often
called as ‘‘macrofibril’’. The cell wall consists of a hollow tube,
which has four different layers: one primary cell wall and three
secondary cell walls and a lumen. The lumen is an open channel
in the centre of the macrofibril. Each layer is composed of cellulose
embedded in a matrix of hemicellulose and lignin [4]. The microfi-
bril is composed of crystalline and amorphous regions alternately,
as is shown in Fig. 2c [4].
The age of the plant, climate conditions and fibre processing
techniques would greatly influence the structure of fibres as well
as their chemical composition. The primary constituents of plant-
based fibres (lignocelluloses) are cellulose, hemicelluloses and lig-
nin. Cellulose contains alcoholic hydroxyl groups so that it is
hydrophilic in nature [4]. The moisture content of plant-based fibre
could reach to 8–12.6% [8]. Cellulose is a highly crystalline struc-
ture which contains as much as 80% of crystalline regions. The
microcrystalline structure of cellulose includes crystalline regions
(higher packing density) of high order, which are extensively dis-
tributed throughout the fibre, and lower order amorphous regions
(lower packing density) [4]. Hemicellulose is made up of highly
branched polysaccharides including glucose, mannose, galactose,
xylose, a group of polysaccharides (excluding pectin) attached to
the cellulose after the removal of pectin. Hemicellulose contains
different types of sugar units. It is also a highly branched polymer
(contrasting with the linear cellulose) and has a degree of polymer-
isation 10–1000 times lower than that of cellulose [4]. Lignin is
amorphous, highly complex, mainly aromatic, polymers of phe-
nyl-propane units [2]. Lignin stiffens the cell walls and acts as a
protective barrier for the cellulose. The function of Lignin is a struc-
tural support material in plants. During synthesis of plant cell
walls, polysaccharides such as cellulose and hemicellulose are laid
down first, and lignin fills the spaces between the polysaccharide
fibres and cementing them together. This lignification process
causes a stiffening of cell walls, and the carbohydrate is protected
from chemical and physical damage [8].
The basic chemical structure of cellulose in all plant-based fi-
bres is similar but they have different degrees of polymerisation
whereas the cell geometry of each type of celluloses varies with
the fibres. These factors contribute to the diverse properties of
the green fibre (Fig. 3).
2.3. Animal-based fibre
An animal fibre generally is comprised of proteins such as col-
lagen and keratin. It can be divided into animal hair and silk. Ani-
mal hair fibre is defined as the fibre which is taken from animals
and hairy mammals. Examples of animal hair are sheep’s wool,
cashmere, alpaca hair, horse hair. Sheep’s Wool is mainly com-
posed of a-keratins, a protein which mainly forms the horny layer
of the epidermis and of epidermal appendages such as hair. Wool is
a multi-component fibre which consists of about 170 different pro-
tein molecules and these protein molecules constitute the morpho-
logical components of wool [9]. The diameter of wool fibre is in the
range of 20–40 lm and the cross-section is elliptical [10]. The wool
fibre is typically divided into three morphological components
including cuticle, cortex and cell membrane. The microfibrils in
the cortex represent approximately 50–60% by mass of the cortex
material, the bonding between the microfibrils and their embed-
ding matrix within the cortex and the presence of the organised
helics within the microfibrils dominate the mechanical and water
absorption properties of wool fibres [11]. Another type of animal
hair is avian fibres, which are feathers and feather fibre. Chicken
 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562 3551

Fig. 1. The classification of different natural fibres.

Table 1
Mechanical properties of natural and man-made fibres.

Fibre Density (g/cm3) Elongation (%) Tensile strength (MPa) Young’s modulus Refs.
Natural fibre
Cotton 1.5–1.6 7.0–8.0 287–597 5.5–12.6 [8]
Jute 1.3 1.5–1.8 393–773 26.5 [8]
Flax 1.5 2.7–3.2 345–1035 27.6 [8]
Hemp 1.6 690 [8]
Ramie 3.6–3.8 400–938 61.4–128 [8]
Sisal 1.5 2.0–2.5 511–635 9.4–22.0 [8]
Coir 1.2 30.0 175 4.0–6.02 [8]
Viscose (cord) 11.4 593 11.0 [8]
Soft wood kraft 1.5 1000 40.0 [8]
Kenaf 1.5 930 53 [10]
Nettle 1.7 650 38 [10]
Abaca 430–760 [10]
Oil palm 0.7–1.55 3.2 248 25 [10]
Pineapple 2.4 170–1627 60–82 [9]
Banna 3 529–914 27–32 [9]
Wool 25–35 120–174 2.3–3.4 [9]
Spider silk 17–18 875–972 11–13 [9]
B. mori silk 1.33 19.55 208.45 6.10 [11]
Twisted B. mori silk 20.57 156.27 3.82 [11]
Tussah silk 1.32 33.48 248.77 5.79 [11]
Man-made fibre
E-glass 2.5 2.5 2000–3500 70.0 [8]
Aramid 1.4 3.3–3.7 3000–3150 63.0–67.0 [8]
Carbon 1.4 1.4–1.8 4000 230.0–240.0 [8]

feathers are approximately 91% protein (keratin), 1% lipids, and 8%
water. Their fibre diameters were found to be in the range of 5–
50 lm [12]. Experimental results have showed that the tensile
strength varies indirectly with the moisture content. The tensile
strength of feather rachis conditioned at 100% relative humidity
was 106 MPa. The tensile strength of feather rachis conditioned
at 0% relative humidity was 221 MPa [12]. The Young’s modulus in-
creased remarkably along the length of the rachis, with the highest
values at the feather tip. X-ray diffraction measurements showed
more keratin molecule orientation further out along the rachis.
Moreover, the fibre located closer to the bird is smaller in diameter
and has lower physical properties compared with the fibre which is
far from the rachis [13]. It is obvious that flight feather fibre exists
in a hollow form while down fibre is in solid. In terms of the pur-
pose of fibre-reinforcement, the use of down fibre appears much
better than that the use of flight fibre [14].
Silk fibre is a type of fibre collected from dried saliva of bugs or
insects during the preparation of cocoons. Silks are generally
defined as protein polymers that are spun into fibres by some
Lepidoptera larvae such as silkworms, spiders, scorpions, mites
3552 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
Fig. 2. (a) Scanning electron micrograh of a kenaf bark fibre, and schematic representations of, (b) macrofibril and (c) microfibril of natural plant [4].
Fig. 3. Properties of cellulose fibres and their dependence on chemical constituents [4].
and flies [15]. Spiders have six or seven sets of glands including
major and minor ampullate, flagelliform, aggregate, cylindrical,
aciniform and piriform for production of fibres with different ami-
no acid composition. These silks serve as: (1) orb-web Frame, (2)
prey capture, (3) wrapping, (4) joint and attachment, (5) reproduc-
tion, (6) vibrational sensor and (7) dispersion [16]. The mechanical
properties of the dragline silk are highly influenced by the compo-
sition of amino acids, insect size, diet conditions, body temperature
and drawing speed. [16] Some spider silks exhibit over 200% elon-
gation. Compare with kevlar fibre, the tensile strength of spider silk
is a factor of four less than kevlar fibre (3.4–4.1 GPa), but the
energy used to break the silk is about three times greater
(1  105 J kg 1) [17]. However, the predatory nature of spider silk
causes it difficult to handle so that the production of spider silk fi-
bre is relatively low compared to silkworm silk fibre [15].
Arthropods including spider and silkworm have evolved to pro-
duce a variety of task-specific silk-protein-based fibre. However,
Silkworm silk fibre is different to the spider silk fibre as only one
type of silk generate by individual silkworm but individual spider
can generate 6–7 types of silk for different purposes. Moreover,
the dragline produced by spider silk cannot yet be produced in suf-
ficient quantity to support any industrial process. Moreover, the
glue-like proteins are generally absent in the spider silk. Therefore,
silkworm silk is found to be a higher potential material used for
industry and medical application.
The silkworm cocoon is built at the end of the larval stage and
protects the pupa during metamorphosis to an adult moth. It
contains silk protein, known as silk fibroin which is stored in the
glands of insects and spiders as an aqueous solution. It is under-
stood that the water is acting as a plasticizing agent, keeping the
protein malleable [18]. Silk protein is usually produced within
specialised glands after biosynthesis in epithelial cells, followed
by secretion into the lumen of these glands and prepared to spin
out as filament [15]. During the spinning, the concentration of silk
in the solution is gradually increased, formation of shear and elon-
gational stresses acting on the fibroin solution in the gland. Elonga-
tional flow orients the fibroin chains, and the fibroin (liquid) is
converted into partly crystalline, insoluble fibrous filaments (solid)
[27]. The bulk of the polymer chains in the crystalline regions are
oriented parallel to the fibre axis [18]. Simpson et al. [19] have
found that the speed of spinning controls the mechanical proper-
ties of fibre.
Silkworm silk, the core filament is an inhomogeneously distrib-
uted polymer blend of mainly two proteins that is coated with gly-
coproteins and lipids [20]. The silkworm cocoon silk fibre is
composed of two cores of fibroin because their gland is a paired or-
gan which surround by a cementing layer of sericin in a structure
known as bave shown in Fig. 4 [21]. The core fibres are encased in a
sericin coat, a family of glue-like proteins that hold two fibroin fi-
bres together to form the composite fibres of the cocoon case [22].
This glue-like proteins is called sericin which is amorphous in
nature and acts as binder to ensure the structural integrity of the
cocoon [23]. The fibroin fibre itself is a bundle of several fibrils
with a diameter of 1 lm. A fibril contains 15 nm wide microfibrils.
 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
Fig. 4. Structure of silkworm silk fibre [21].
Microfibrils are packed together to form the fibril bundle and sev-
eral fibril bundles produce a single strand [23,24].
The convenience of reeling long (300–1200) continuous fibre
from the cocoon has certainly contributed to its success as a tex-
tile fibre. However, a long and continuous fibre can only be reeled
from the cocoon after the adhesive sericin coating is removed.
Sericin removal requires thermo-chemical treatment of the co-
coon in a process conventionally known as degumming [21].
However, degumming would weaken at least one type of non-
covalent interaction of core fibroin, such as hydrogen bonds and
Van der Waal’s bonds. The two important factors associated with
degumming could affect the tensile properties of silkworm silk
because of the change in the microstructure of two core fibroins
[22].
Fig. 5. Cross section, longitudinal view and perspective of silk filaments.
3553
Compared with the commercially Mulberry silkworm silk (Bom-
byx mori), Tussah silk is a textured silk with the brownish toned. It
is mainly due to tannin from the variety of trees fed by the
caterpillars. Most silkworm cocoon and spider dragline silk fibres
contain assembled anti-parallel b-pleated sheet crystalline struc-
tures. Silks are considered semi-crystalline materials with 30–
50% crystallinity in spider silks, 62–65% in cocoon silk fibroin from
the silkworm B. mori, and 50–63% in wild-type silkworm cocoons
[27]. Fig. 5 shows the cross section, longitudinal view and perspec-
tive of silk filaments.
2.4. Biodegradable polymers
Conventional polymers such as polyethylene (PE) and polypro-
pylene (PP) are used for many years and have been developed to be
an absolutely necessary part of our life in almost every area
nowadays. With time and the rapid development of science and
technology, the mechanical property, stability and durability of
conventional polymers have been improved continuously. How-
ever, these long lasting polymers seem inappropriate in application
of the product which has short product life cycle, such as plastic
plates and fork for party. These polymers persist for hundred years
in a landfill after disposal. Therefore, advantages as disadvantage,
high durable property of these polymers increase the environmen-
tal burden. Moreover, these polymers are often disposed and
stained with food residue; increase the complexity of the plastic
recycling. The cost of recycling of plastic is thus so high and so that
there is no choose to land filling or incineration of plastic. As the
public starts focusing on the huge environmental accumulation
of these long lasting polymers and pollution problem caused dur-
ing and after the life cycle of the polymers (such as manufacturing
and disposal process), and fitting the modern society, the study on
naturally-degradable polymers with short life cycle is needed.
Biodegradable polymers were first introduced in 1980s [25]
which are designed to degrade upon disposal by the action of
microorganisms. In general, polymers are solid, non-metallic
compounds with high molecular weight. They are comprised of re-
peated marcomolecules, and have varying characteristics. Material
usage and final mode of biodegradation are dependent on the com-
position and processing method employed [26]. These polymers
means capable of undergoing decomposition into carbon dioxide,
methane water, inorganic compounds or biomass in which the pre-
dominant mechanisms is the enzymatic action of micro-organisms
that can be measured by standard tests, over a specific period of
time, reflecting available disposal conditions.
3554 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562

These polymers can be also classified on the basis of the origin,
that is, naturally occurring or synthetic in Fig. 6 [27]. Natural poly-
mers are available in large quantities from renewable sources,
while synthetic polymers are produced from non-renewable petro-
leum-based resources. Nowadays, degradable polymers used in
various forms including films, moulded articles, sheet, etc. The po-
tential applications of biodegradable applications include: (1) film
such as plastic shopping bags and bin bags, (2) cling wrap, (3)
flushable sanitary products, (4) sheet and non-woven packaging,
(5) bottles and container, (6) loose fill foam and (7) medical appli-
cation. Among these biodegradable polymers, aliphatic polyesters
constitute the most attractive family have been extensively stud-
ied. Table 2 summarizes the properties of aliphatic polyesters.
Polyesters play a predominant role as biodegradable plastics due
to their potentially hydrolysable ester bonds.
Poly (lactic acid) (PLA) belongs to the family of aliphatic polyes-
ters derived from a-hydroxy acids. PLA is a compostable polymer
derived from renewable sources which is mainly from starch and
sugar. Since PLA is compostable and derived from sustainable
sources, it has been viewed as a promising material to reduce soci-
etal solid waste disposal problems [28]. A high-molecular PLA can-
not be directly synthesised from the molecule of lactic acid, mainly

Fig. 6. Natural and synthetic biodegradable polymers [27].

Table 2
The properties of aliphatic polyesters.

Examples Crystallinity Glass transition Melting Modulus Loss strength Loss mass Processing Refs.
temp. point (month) (month) temp.
Poly (butylene succinate) (PBS) 45 to 10 90–120 0.4–0.6 160–200 [32,38]
Poly(ethylene succinate) (PES) 45 to 10 90–120 160–200
Polyglycolide (PGA) 45–55% 35–40 200 12.5 Gpa 1–2 6–12 [38]
Polycaprolactone (PCL) 67 -60 55–60 0.19 24–36 [38–40]
Polylactides
Poly L-lactide (PLLA) 37 60–65 170–180 4.8 6 12–24 [38,39]
Poly D-lactide (PDLA)
Poly DL-lactide (PDLLA) 55–60 1.9 1–2 12–16 [38]
Polydioxanone PDS, PPDO High <20 2.1 1.5 1–2 6–12 [38,35,42]
Poly hydroxyalkanoates PHA
Poly(3-hydroxybutyrate) (PHB) 80 5 173–180 0.9–4 [40,41]
PHV
PHH
Poly(trimethylene carbonate) PTMC 3–4 [38]
 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
because of the generation of water during the condensation pro-
cess (leading to the degradation of the PLA formed and formation
of only low-molecular oligomer). In general, three different ways
can be followed to solve this problem:
(1) Addition of chain-coupling agents during the condensation
process.
(2) Dimerization the oligomer into cyclic lactide (see above),
distillation of solution to take out the water condensed
and then production of the PLA by ring-opening
polymerisation.
(3) Azeotropical dehydration during the condensation process,
removing the water during the process by change of
pressure.
PLA belongs to the family of the polyester and is generally linear
(without strong entanglement, branching between the chains). The
structure of the molecule influences its mechanical and thermal
properties (for PLA 3051D: Tg is 55–65 °C, Tc 150–165 °C and ten-
sile strength 48 MPa [29]), which are quite similar to other poly-
esters (such as PET). The thermal properties are however a bit
lower, due to the absence of the benzoic cycle (chain more free
to move). Its chemical properties and water resistance are weak-
ened by the presence of the carbonyl group (C@O), which allows
hydrolysis degradation. Like most of the polymers, the different
macromolecules (chains) are bonded together by hydrogen bonds
(Van de Waals forces). Most important mechanical and thermal
properties (crystallinity rate, Tg and Tm) are then influenced by
the concentration and disposition of different enantiomers (L-
and/or D-lactic acid). Indeed, the chains made of a unique basic ele-
ment can align each other easier in a configuration favoring inter
chain bonds. Thus the lowest Tg is found in racemic mixing of L-
and D-enantiomers while the highest properties are obtained by
stereo complex PDLA and PLLA blends (respectively using the D-
and L-enantiomers) and reach a maximum with a ratio of 50:50.
Like most polymers, PLA is hydrophobic. It can only absorb 1%
water content and undergo hydrolytic degradation, making it bio-
degradable and environmentally friendly. PLA normally undergoes
three main degradation processes: (i) chemical hydrolysis, (ii)
enzymatic degradation and/or (iii) microbial degradation [30].
During chemical hydrolysis, the water molecule attacks the double
bounding C@O of the PLA, like shown below:
The enzymatic degradation occurs mainly in the amorphous re-
gion of the polymer and seems to attack preferentially the ester
bonds of L-lactic acid (cleaving the polymer). The PLA-degrading
and the silk fibroin-degrading enzymes belong roughly to the same
groups and it seems that the L-lactic acid unit of PLA is recognised
as similar to the L-alanine unit of silk fibroin. The same conclusion
can be made for the microbial degradation, where the bacteria’s
ability to degrade the PLA and silk are linkable. One can moreover
note that the bacteria able to degrade PLA are more scarce than the
ones able to degrade most of others polyesters [15].
In order for PLA to be processed on large-scale production lines
in applications such as injection moulding, blow moulding, ther-
moforming, and extrusion, the polymer must possess adequate
thermal stability to prevent degradation and maintain molecular
weight and properties. PLA undergoes thermal degradation at tem-
peratures above 200 °C (392.8 °F) by hydrolysis, lactide reforma-
tion, oxidative main chain scission, and inter- or intra-molecular
transesterification reactions. PLA homopolymers have a glass tran-
sition and melt temperature at about 55 °C and 175 °C, respec-
tively. They require processing temperatures over 180 °C. At this
temperature, unzipping and chain scission reactions leading to loss
of molecular weight, as well as thermal degradations, are known to
occur. Consequently, PLA homopolymers have a very narrow pro-
cessing window. The rheological properties of PLA, especially the
3555
shear viscosity, have important effects on thermal processes, such
as injection moulding, extrusion, film blowing, sheet forming, fibre
spinning, and thermoforming. Poly-Lactide melts are shear thin-
ning, similar to polystyrene. Its working temperature is dependent
on the melt viscosity, which is, in turn, dependent on the weight-
average molecular weight of PLA, the amount of plasticizer, the
shear rate, the type of melt processing, and the amount of work
put into the polymer. Under the same processing conditions,
semi-crystalline PLA had a higher shear viscosity than amorphous
PLA. As the temperature increased, the shear viscosity decreased
for both types of PLA. The PLA melt was characterised as a pseudo
plastic, non-Newtonian fluid [31].
3. Processing of raw materials
3.1. Selection criteria
Suitable manufacturing processes must be utilised to transform
the materials to the final shape without causing any defect of prod-
ucts. For the selection a suitable process to fabricate biodegradable
polymer-related composites, design and manufacturing engineers
would mainly focus on numbers of criteria including desired prop-
erties, size and shape of resultant composites, processing character-
istics of raw materials, the production speed and the manufacturing
cost. The size of the composites is a dominating factor for the pre-
liminary assessment on a suitable type of manufacturing processes
to be used. For small to medium sized components, injection and
compression mouldings are preferred due to their simplicity and
fast processing cycle. However, for large structures, they are typi-
cally manufactured by open moulding and autoclave processes.
Similar to other plastic products, the complexity of shape of a prod-
uct also influences the type of manufacturing processes to be used.
For example, filament winding is the most suitable method for
manufacturing composites pressure vessels and cylinders. Recent
development has also used carbon fibre wrapped on the surface
of forged Aluminium cylinders to form ultra-high pressure tanks.
Pultrusion is mainly used for producing long and uniform cross-
section parts. In some extent, optic fibre can be integrated into the
pultrusion process to produce self-structural-health monitored
composite structures. The shape of the parts being made is highly
dependent on the shape of the die. Somehow, several stages of heat
control are needed to cure the composite parts. Depending on the
performance of composites products, suitable raw materials (ther-
mosets/thermoplastics, high/low viscosity, processing tempera-
ture) should be chosen with an appropriate composite fabrication
technology.
However, in certain extent, the criteria of selecting the right
manufacturing processes for natural fibre composites are different
with that to be used for traditional polymers. The properties of nat-
ural fibre composites are highly dependent on the length, orienta-
tion, diameter and content of fibre. The surface condition of the
fibre also plays a key role as it would affect the bonding interface
between the fibre and surrounding matrix. Removal of a surface
coating of fibre (like silk and coir fibres) or pretreatment of fibre
(like hemp) by using chemical process may be needed to ensure
a good bonding is resulted. Theoretically, high tensile strength
could be achieved by increasing the amount of fibre used. How-
ever, it may not be done by using injection moulding process as
the expansion of fibre in wet condition could cause a sucking ef-
fect. Therefore, compression moulding may be used for a simple
form of composites products.
Natural fibres extracted from wool and cocoon silks are com-
prised of numerous of micro-fibrils. It has been reported that these
fibres after degumming, only two triangular fibrils (brins) would
be remained, and these fibrils are formed by several thousands of
3556 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
Fig. 7. Scanning electron micrographs showing the micro fibrils of the silk inside the composites.
micro-fibrils as shown in Fig. 7. A noteworthy weakness in the nat-
ural fibre reinforced thermoplastic composites is the poor interfa-
cial bonding between the fibre and matrix. The interfacial adhesion
between them plays an important role in determining the perfor-
mance of the composites. This is mainly due to their dissimilar
hydrophobicity as the surface of fibre is hydrophilic while organic
plastics are generally hydrophobic, they are incompatible and pre-
vent efficient fibre–matrix bonding. The incorporation of hydro-
philic fibres in polymers leads to heterogeneous systems whose
properties are inferior due to poor adhesion between the fibres
and the matrix [32–34]. Therefore, these debonded fibres dilute
the matrix content and act as flaws which reduce the effective
cross sectional area and, finally poor mechanical strength is re-
sulted. Moreover, the formation of fibres agglomeration, due to
the inter-fibre hydrogen bonding which prevents thorough disper-
sion of fibres during the manufacturing process and thus weakens
the strength and affects the appearance of the composites [32,35].
Thus the treatment of natural fibres for adhesion improvement
is a critical step in the development of the composites. Different
treatments such as pre-impregnation, surface modifications,
chemical reactions and plasma have been studied for interfacial
shear strength improvement in order to develop composites with
better mechanical properties [32,33,36–38]. Natural fibre always
cannot be wetted completely by following the general manufactur-
ing processes as they are not designed for wetting fibre with tight-
packing fibrils. The viscosity of polymers is normally too high for
impregnation. Better fibre pre-impregnation allows a better fibre
wetting and thus enhances the mechanical interlocking between
fibre and matrix [36].
The surface modifications of fibres by using compatibilizer or
coupling agent for effective stress transfer across the interface
were explored. The compatibilizer is a kind of polymeric interfacial
agent or polymers with functional groups that graft onto the chain
of polymers. Besides, coupling agent is a chemical substance which
is able to react chemically on the both natural fibre and the poly-
mer matrix during processing to form or promote a stronger bond
at the interface as bridges in order to improve the mechanical
properties of resultant composites. The nature of bond formed be-
tween a specific coupling agent and fibres depends strongly on the
characteristics of the fibre surface to which the coupling agent is
adhered [32]. The coupling agents are tetrafunctional organome-
tallic compounds which are commonly known as silane, zirconate,
or titanate coupling agents [33]. Rozli Zulkifli et al. [38] have found
that the silk/epoxy composite with fibre surfaces which treated by
silane-based coupling agent shown an improvement of the adhe-
sion. Keener and Stuart [34] used polyethylene couplers and the
results indicated that the tensile strength and impact property of
the coupled composites were improved as compared with non-
coupled blend composites. Kazayawoko et al. [35] used Maleated
polypropylene (MAPP) as a coupling agent and the effectiveness
of MAPP has been attributed to its ability to wet and disperse the
wood fibre efficiently.
Chemical treatments such as dewaxing, delignification, acetyla-
tion, and chemical grafting are used to modify the surface proper-
ties of the fibres and enhance the performance of composites [33].
Alkaline processing is one of the most common chemical treat-
ments in the industry which are not only used for increasing the
surface roughness of the natural fibre that results in a better
mechanical interlocking, but also for the increments of the amount
of cellulose exposed on the plant fibre surface, thus increasing the
number of possible reaction sites. Valadez-Gonzaleza et al. [36]
have explored the fibre–matrix interphase physicochemical inter-
actions of the natural fibre reinforced plastic. They have found that
the fibre surface area was increased by the means of alkaline
treatment.
Plasma treatment is an environmentally-friendly new technol-
ogy which can alter the surface properties of the materials without
interfering their bulk properties. Chaivan et al. [36] have studied
the utilisation of SF6 plasma treatment for improvement in hydro-
phobic property of silk fibre. A reproducible and significant in-
crease in the hydrophobic property compared with the untreated
sample was obtained.
4. Moulding processes
4.1. Injection moulding
Injection moulding of composites is a process that forces a mea-
sured amount of mixture which contains molten polymer and fibre
into mould cavities. Many studies have been conducted on the po-
tential of using natural fibres as reinforcement for renewable poly-
mers to make a composite through injection moulding [40–45].
The original thermoplastic polymer used by this process was
designed for plastic pellets. For fibre reinforced composites, the
pellets with chopped fibres are fed individually through a funnel-
shaped feed hopper into a heated compression barrel with a
rotating screw (‘‘screws’’ for twin-screw extruder). The purpose
of heating the barrel is to transform the solid pellets into viscous
liquid which can be drove through the sprue nozzle and finally
forced into the matched-metal closed mould cavities. The mould
is tightly clamped against injection pressure where the polymer
solidifies, freezing the orientation and distribution of fibres. The
composite is then removed from the closed mould after it is suffi-
ciently cooled to be ejected to form a part of desired shape. As the
mixture is required to move toward to the sprue nozzle, polymer is
pressurised because of the screw mechanism. The function of the
screw is to (1) generate heat by viscous shearing to melt the
 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
polymer, some heat that is used for melting pellets evolved from
the friction in between pellets, barrel and screw [45], (2) apply
the shear force to mix the polymer and fibre and (3) act as a piston
to force the mixture of fibres and molten polymer through sprue
nozzle into a matched-metal closed mould. It has been reported
that as the temperature increases, the shear viscosity of biodegrad-
able polymers would decrease which makes the flow easier. Be-
sides, as the shear rate increases, the viscosity of the polymer
melts would also be decreased significantly. This change of viscos-
ity is caused mainly by the breaking of PLA molecule chains due to
the strong shear forces and temperature [46].
Fibre that is used in the injection moulding is usually chopped
into short fibre according to the critical fibre length criterion in
which the stress should be fully transferred from the matrix to
the fibre and the fibre can be loaded to its full capacity assuming
a good interfacial bonding is resulted. However, the traditional
injection moulding process limits the fibre length that solidifies
in the final part since the high shear rates in the barrel and the pas-
sage of fibres through narrow gates and openings in the mould
which cause significant fibre attrition. Therefore, the fibre length
in practice is normally shorter than the predicted fibre length be-
cause of the fibre attrition. This fibre attrition causes the fibre
length below the critical length as expected, the fibres shorter than
the critical length would not be able to carry their maximum load
effectively. In an extreme case, the fibre rather acts as a defect in
the material not only because of its length effect, but also on the
poor bonding properties. Nevertheless, if the fibre length is beyond
the pre-determined critical length, it will carry an increasing frac-
tion of the applied load and may fracture prior to the failure of the
matrix. Therefore, it is necessary to carefully determine the critical
length of the fibre before injection moulding is performed. On the
other hand, increasing fibre content would theoretically improve
the stiffness and the strength of resultant composites. However,
in practice, the traditional injection modelling process would limit
the amount of fibres to be injected because of the fibre cluttering,
narrow gate and sprue and, viscosity of the fibre/polymer mixture.
Another main issue is the volume expansion of the fibre after mix-
ing with the liquid form of matrix.
Residual stress and fibre orientation with respect to the depth
are also the critical issues which affect the modulus distribution
of the injection moulded composites. Residual stress is an internal
stress which occurs as a result of the rapidly cooling of molten
polymer in the absence of external forces. In general, the residual
stress distribution shows tensile stresses at the surface and core re-
gions and compressive stress at the intermediate region, which is
well-known as the characteristic residual stress distribution in
injection-moulded parts [47]. Numerous of researches have there-
fore studied the residual stress distribution of composites made by
the injection moulding process [46–49]. (1) High pressure gradient,
(2) non-uniform temperature profile caused by inhomogeneous
cooling of the polymer melt, (3) orientation of polymer chains
and (4) the difference in thermal expansion coefficient between
matrix and fibres are the common phenomena which residual
stresses may be introduced in injection moulded polymers or com-
posites during filling, packing, and cooling stages.
When the flow is ceased, the molecule orientation starts to relax
while solidification process subsequently occurs before this pro-
cess is completed. It would impede the relaxation of the molecular
orientation which is then frozen in, the residual stress is therefore
formed inside the part. Residual stress in a pure thermoplastic
polymer and its fibre composites cause an earlier fracture of the
composites which affect the quality of products seriously. Stress
distribution along the flow path is influenced by the pressure his-
tory of the molten mixture at the beginning of the injection mould-
ing process to the end of filling up the mould cavity. The various
features of the stress profiles are explained by the influence of
3557
the pressure decay rate in the injection-moulding process [49].
These residual stresses also result in warpage and shrinkage of
the final products and may induce reduction of mechanical proper-
ties. Therefore, the dimensional accuracy and properties of the final
products are highly related to the residual stress distribution in the
moulded part [47]. For natural fibres, as their moisture absorption
characteristics, impurities and voids formation inside injection
moulded composites may be resulted as high temperature is used
during the process and cause water molecules trapped inside mi-
cro-fibrils to be gasified.
Fibre orientation in an injection moulded short fibre composite
is experienced variation with respect to the thickness direction as
well as the in-plane direction. It induces the mechanical properties
of the composite such as modulus and tensile strength may vary in
the thickness direction according to the corresponding orientation
status. For the range of fibre concentrations encountered commer-
cially, fibres do not appear to have any direct effect on the matrix
orientation. As the fibre concentration increases, however, the ma-
trix orientation becomes dominated by the orientation of the fibres
[50]. During the injection moulding process for composites, a com-
plex molten polymer flow field is generated and fibres are there-
fore oriented. The orientation of fibres will be fixed until the
matrix is solidified. Convergent flow results in high fibre alignment
along the flow direction, whereas diverging flow causes the fibres
to align at 90° to the major flow direction. Shear flow produces a
decrease in alignment parallel to the flow direction and the effect
is pronounced at low flow rates. In generally, the fibres align in
the direction of shearing and also in the direction of stretching.
The shear flow near the mould walls aligns the fibres in the direc-
tion of the injection flow and this layer is called the skin. Below the
skin layer, the molten mixture continues to experience shear and
fibres orient along the shear lines. Finally, the core layer is formed
as the fibres are swayed by the bulk deformation of the flow in the
mould which usually has an elongated component, causing the
material to stretch in and out of the paper direction aligning the fi-
bres. This skin core structure shown in Fig. 8 is a common micro-
structural observation [48,51]. However, the skin core structure
is less significant in the small sample with low fibre volume frac-
tion. To assess the alignment of fibres during the manufacturing
process in a small sample, small and thin dumbbell shaped com-
posite samples were made by injection moulding. A microscopy
was used accordingly to observe the fibre orientation through
the image analysis technique. According to Fig. 9, most of the fibres
are well aligned along the sample’s axis (i.e. the loading direction),
only a small amount of obliqued fibres.
There are numerous issues that should be concern during the
injection moulding process to obtain the optimal properties of
the resulting natural fibre composites and avoid development of
residual stress which cause warpage, stress cracking, and long-
term deformation. Process, material and geometric parameters
should be optimised to minimise these problems happen. Process
parameters include the melt temperature, injection and screw
speeds, injection pressure and the mould temperature that can
be controlled on the injection units. Increasing mould temperature
results in a decreasing overall stress level, while the compressive
stress region is shifted onto the surface [49]. According to recent
research investigations, for biocomposites, the machine tempera-
ture of biodegradable polymer, such as Poly-lactic-acid (PLA) com-
posites was made by using injection moulding process should be
restricted in the range of 150–210 °C depending on the type of
PLAs and their crystallinity from diverse manufacturers.
Molten polymer rheology, and fibre type and content are the
material parameters which affect the manufacturing process and
the properties of resultant composites. Under the same processing
conditions, semicrystalline PLA had a higher shear viscosity than
that of amorphous PLA [46]. The geometric parameters also play
3558 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562

Fig. 8. Micro graphs of cut-off view (along the longitudinal direction of the sample) of the silk fibre/PLA composite with 5 vol.% silk fibre: (a) wide section and (b) narrow
section.

Fig. 9. Influence of flow on fibre orientation: Skin-fibres are mostly aligned along the flow direction; Core-fibres are mostly aligned perpendicular to the flow direction.

a key role on the residual stress elimination. The mould cavity
shape and size, the locations of injection gates and the vents that
allow the air to escape are the examples of geometric parameter
which not only affect the residual stress, but also the air trapping
and stress concentration.
4.2. Compression moulding
Many studies have been conducted on the feasibility of using
natural fibres as reinforcement mixed with renewable polymers
to form a new class of biocomposites through compression mould-
ing process [40–44]. This process is a combination of hot-press and
autoclave processes. For autoclave process, thermoplastic prepregs
are laid up on a mould in a desired sequence. An entire laminate is
then bagged under vacuum and placed inside an autoclave. The
laminate is then heated up following a preset heat-pressure cycle
and a resultant composite is formed after curing [52]. However,
for the hot-press processing, a close mould may or may not be nec-
essary [53]. With the use of close-moulds, the precut and weighed
amount of fibres (in the forms of chopped, mat or stitched) are
stacked together and placed inside a pre-heated mould cavity.
For natural fibre, the fracture of some fibres may occur before resin
films are molten if excessive pressure is applied. Sheet moulding
compounds (SMCs) and bulk moulding compounds (BMCs) are tra-
ditional initial charges for compression moulding process. The
charges usually cover 30–70% of the female mould cavity surface
[52]. The mould is closed and then pressurised before temperature
is applied. The compounds are molten to form the shape of the cav-
ity. Afterward, the mould is opened and the part is ejected. As the
fibre can be gently placed inside the mould and no shear stress and
vigorous motion are applied, the damage of the fibre can be kept as
minimal. In this case, long fibre can be used to produce a biocom-
posites with higher volume fracture. For the natural fibre compos-
ites, short fibres or fibre mats could be pre-mixed with the
compounds for compression moulding, it would act as reinforce-
ment to reduce the shrinkage of final products.
4.3. Hot pressing
As mentioned in the previous section, hot press is favourable
for simple flat samples as only two hot plates are needed to
compress all fibre and matrix together and then heat was applied
 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
subsequently. However, the viscosity of the matrix during the
pressing and heating processes is a concern as it is not easy to
be controlled, in particular for think samples. The viscosity of
the molten matrix should be low enough to impregnate into the
space between fibres and high enough to avoid spurting out. As
natural fibres are made by many small filaments, it also takes
time for wetting them. Therefore, the controls of viscosity, pres-
sure, holding time, temperature in relation to the types of fibres
and matrix, thickness and size of samples are critical to produce
quality composites. Several minor defects such as residual stres-
ses, voids, warpage, fibre breakage, sink marks and scorching
would cause the reduction of the mechanical properties of the
composites. Therefore, process, material and geometric parame-
ters should be optimised to minimise possible defects appear.
One more critical issue is, for biodegradable polymers, their pro-
cessing temperature is normally below 200 °C to avoid the degra-
dation of the polymers. If the products are thick, the heat is
required to be transferred from the surfaces of the products to-
ward the core. Carefully studying the temperature gradient is
essential to avoid overheating on the surface or sub-temperature
in the core to melt the polymers.
Based on the past experience, it was found that the tensile prop-
erties of natural fibre composites decrease when the set mould
temperature and flow velocity decrease. Most of natural fibres
are normally distributed randomly at the beginning and finally
aligned toward the matrix flow direction for flat plate moulding
[54,55]. The required temperature and pressure for the moulding
process may be varied depending upon the thermal and rheological
properties of the matrix. Flow of the material is required to expel
air entrapped in the mould as well as in the charge. Void morphol-
ogy in the sample has a negative effect on the flexural modulus and
strength, but a clear positive effect on the beam stiffness [56]. Dur-
ing the moulding process, a complex heat transfer and a viscous
flow phenomenon take place in the cavity [57]. For a good moulded
part, a rapid mould-closing speed is desirable since it avoids the
possibility of premature gelation and produces most uniform flow
patterns regardless of the charge thickness [52].
Material parameters, for example, increasing the filler content
also acts as a heat sink within inside the material as it would de-
crease the total amount of heat liberated [52]. The initial charge
shape, size and its placement location in the mould are crucial
parameters as they influence the final properties of a product.
The amount of flow in compression moulding is small but critical
to the properties and the quality of final parts because the flow
controls the orientation of short fibres which is the main factor
to determine the physical and mechanical properties of a resultant
composite. To help control the moulding process smoothly and
effectively, an optimised fibre which possesses high-surface en-
ergy, a low expansion, and low swelling should be used so as to
lead to a better wetting and impregnation [58].
A slight excess of material is usually placed inside the mould to
ensure it is completely filled. It is possible to have varying degrees
of flow of fibres and/or of melt in compression moulding, the fibres
are initially randomly oriented. However, as the mixture becomes
fluid in the mould it deforms and the deformation changes the ori-
entation of the fibres. Orientation distributions can be extremely
complicated. Some locations the fibre can retain at randomly ori-
ented, whereas others may have high degree of alignment toward
the flow direction. Increasing the fibre content also leads to
enhance the anisotropy of final moulding products [59]. A low-
viscosity paste may flow too rapidly and cause air entrapment
[58]. Different temperatures inside moulded parts would generate
different degrees of residual stresses, particular at think sections.
Thus, the temperature distribution and rate of cooling are impor-
tant in determining how these stresses relax during cooling status
[54].
3559
The geometry of the moulding part is important which affects
the flowing behaviour and fibre orientation. Fibre content inside
the rib and around the sharp turning sections is normally much
lower than that of other flat sections. It was also found that the
larger the rib thickness, the easier the flow (with the fibres) into
the ribs. However, a small lead-in radius would reduce the flow
or increase the flow resistance into the ribs [60]. High pressure
loss at the entrance of the rib is due to viscous friction. This pres-
sure loss will result in fibre–matrix separation in these areas
which in turn would weaken the structural integrity of resultant
parts and lead to increased sink-mark depth. For the curing pro-
cess concerned, the material at the centre of the rib sub-structure
cures relatively slower than other flat-plate sections. The fibres
are dense near to the top surface and around the rib corners,
whilst a resin-rich area appeared just below the top surface at
the centre [57].) High pressures are required for moulding parts
that contain deep ribs and bosses [52]. Thick structures are not
easily produced by this technique because of heat conduction.
The charge surface temperature quickly attains to the mould tem-
perature and remains relatively uniform compared with the
centreline temperature. The centreline temperature increases
slowly until the curing reaction is initiated at the mid-thickness
of the part. For thin parts, the temperature rise is nearly uniform
across the thickness and the maximum temperature in the mate-
rial seldom exceeds the mould temperature. When the SMCs are
placed at the room temperature on the hot mould, the surface of
the SMCs soften and make them forming a resin-rich lubricating
layer. Thus, for the purposes of modelling, the flow field can be
divided into two regions: the core, which occupies most of the
flow domain: and a thin lubricating layer. This is shown schemat-
ically in Fig. 10 [61]. For a thin part, the extensional deformation
becomes more uniform and approaches the same flow pattern ob-
served at fast mould-closing speeds [52]. For a thick part, high
moulding temperatures should be avoided. Since the surface tem-
perature first attains to the resin gel temperature, curing begins
first at the surface and progresses inward. Curing occurs more
rapidly at higher mould temperature but the peak exotherm tem-
perature also increases [1 0 0]. Residual curing stresses in the
moulded part are reduced as the thermal gradient remains nearly
constant across the thickness through preheating [52].
4.4. Resin transfer moulding (RTM)
Liquid composite moulding processes encompass resin transfer
moulding (RTM), vacuum assisted resin transfer moulding
(VARTM), structural reaction injection moulding (S-RIM), co-injec-
tion resin transfer moulding (CIRTM) and other subsets where the
basic approach is to separately inject the liquid resin into a bed of
stationary preforms. The RTM process has become a popular com-
posite manufacturing process due to its capability for high volume
Fig. 10. Transverse velocity profile for ‘‘Preferential flow’’ [61].
3560 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
Table 3
Common applications of natural fibre reinforced composites.
Potential application Examples
Automotive Door panels, seat backs, headliners, dash boards, car
door, Transport pallets, trunk liners, Decking, rear
parcel shelves, spare tyre covers, other interior trim,
spare-wheel pan, trim bin
Aircraft Interior panelling
Construction Railing, bridge, siding profiles
Household products Table, chair, fencing elements, Door panels, interior
and furniture panelling, Window frames, door-frame profiles, food
tray, partition
Electrical and Mobile cases, laptops cases
electronics
Sports and leisure Sports and leisure items: Tennis Racket, bicycle,
items Frames, Snowboards
production and cost effectiveness. Many studies have been made
on the potential of natural fibres as reinforcement with renewable
polymers as matrix through RTM [62–67]. In the RTM process, dry
fibre perform (impregnating) or porous fibrous preform is placed
into the mould cavity. Two matching mould halves are clamped
tightly to avoid leakage of resin during injection process. Then,
using dispensing equipment, a pressurised molten plastic is in-
jected into the heated mould using single or multiple inlet ports
in the mould depending on the complexity of the shape of a final
product until the mould is filled with resin. After cooling, the part
is then removed from the mould [62]. Post-curing normally is
needed to ensure the resin is fully cured (chemically reacted be-
tween the resin and its catalyst).
In the RTM process, the resin injection pressure, temperature of
the mould, permeability of the fibre mat, preform architecture and
permeability, resin viscosity, gate location and configuration, vent
control and preform placement techniques are the major process-
ing variables. In general, higher injection pressure and mould tem-
perature would shorten the manufacturing cycle time due to the
viscosity of resin is low. However, an excessive injection pressure
may cause deformation of the mould and wash-out of the fibre
preform. An excessively high mould temperature may induce
pre-mature resin gelation and cause short shot. All of the process
variables are interrelated and have effects on the mechanical prop-
erties of final products. These processing variables have significant
effects on different aspects, such as fibre wetting out and impreg-
nation, injection gate design, ‘‘dry patch’’ and void formation [68].
For natural fibre composites, small clearances may exist
between the fibre preform and mould edges because of loose edge
fibre bundles, poor fitting size, or deformation of the fibre preform
in the RTM process. The clearance results in a preferential resin
flow path during the mould filling stage. This edge flow can disrupt
the uniformity of the flow pattern and cause incomplete wetting of
the preform. This phenomenon intensifies with the decrease of
preform permeability. At an early stage of the injection process,
the velocity differences are very high and then gradually reduce.
This is due to the gradual increase in flow resistance which leads
to smaller differences in velocity. Edge flow is introduced due to
the clearance between the preform and the mould edge. The pres-
ence of edge flow leads to the interruption of flow uniformity and
the resin near the edge has a tendency to flow much faster than in
the main area due to lower resistance. Edge flow is less sensitive to
injection pressure variations but fibre concentrations have a dra-
matic influence. The deployment of preforms larger than the
mould eliminates the problem. ‘‘Quasi-one-dimensional steady’’
flow is preferred in order to achieve successful mould filling with
complete impregnation and proper ventilation [69].
For fast resin flow without increasing injection pressure, resin
can be injected using multiple injection gates. However, with im-
proper injection schemes, the resin front becomes complicated
and numerous air bubbles may form where the flow fronts merge
[68]. Because of the high flow resistance and slow flow and
impregnation, the resin has a tendency to flow along the channel
of least resistance under injection pressure and therefore the effect
is intensified. Consequently both the values of mould filling dis-
tance differences between the centre and edge and the arrival time
of edge flow at the bottom are substantially increased. The edge
flow has an adverse effect on the mould filling process which leads
to the formation of dry spots and spillage [70]. Due to aforemen-
tioned problems, it would induce a difficulty to assure full wetting
inside the preform because of the inconsistence of the geometry of
natural fibre and inhomogeneous fibre architecture. Such inhomo-
geneity leads to non-uniform permeability of the fibre preform,
which in turn causes the resin velocity to vary from point to point
at a micro scale. The capillary pressure, which also prevails at this
length scale, exacerbates the spatial variation of the resin velocity.
The resulting microscopic perturbations in the resin flow front al-
low voids to form [71].
While the average velocity field of the resin may appear smooth,
the local velocity can vary considerably from point to point at the
micro scale. The reason is that the fibre preform has a non-uniform
microstructure, and hence its local permeability and the local cap-
illary pressure may differ between inside and outside fibre tows
[71]. It has been shown that there is a marked increase in voidage
in the areas where flows meet and this is correlated to a deteriora-
tion of mechanical properties. The void content within a composite
material produced by RTM will depend on the void content of the
resin prior to injection and the extent of void formation and growth
during mould filling and cure. In general, vacuuming of the mould
and injection pot are required prior to the injection process starts.
5. Potential applications
5.1. Ecological applications
Recent increase of the prices of petroleum-based products,
strict governmental regulations and taxation systems on carbon
footprints and well-educated young generation on the acceptance
of adopting green products have driven the growth of developing
materials with the use of natural resource to another peak. It there-
fore creates a new business model for all engineering enterprises to
re-invent their capital including human resource to adopt this new
change. The application of natural fibre reinforced polymer com-
posites and natural-based resins for replacing existing synthetic
polymer or glass fibre reinforced materials is huge. Automotive
and aircraft industries have been actively developing different
kinds of natural fibres, mainly on hemp, flax and sisal and bioresins
systems for their interior components. High specific properties
with lower prices of natural fibre composites are making it attrac-
tive for various applications. According to Lucintel, a leading global
management consulting and market research firm, the global nat-
ural fibre composites market reached to US $2.1 billion in 2010.
This market is expected to grow with a CAGR (compound annual
growth rate) of 10% over the next 5 years (2011–2016) [72]. Now-
adays, new construction materials using natural fibre are well sui-
ted for anisotropic and specially tailored lightweight structural
components parts such as interior panels inside cars, partitions
(or called ’’dividers’’) inside airplanes and coats and other second-
ary structures with low temperature servicing condition. Table 3
summarizes the potential applications of natural fibre composites
in automotive, electrical and electronics, sports and leisure items,
construction, aircraft and household products & furniture indus-
tries [73–75]. Besides, as natural fibre is formed by several thou-
sands of fibrils together which is an idea structure for energy
absorption including sound wave energy, so it is good for best
 M.-p. Ho et al. / Composites: Part B 43 (2012) 3549–3562
using its inherent advantage for developing noise barriers and im-
pact resistance structures. Moreover, eco-friendly measures taken
by the electronic industry is another major growth driver for these
composites in electrical and electronics applications. Recently, a
major research focus on natural fibre composites, mainly on the
plane-based fibre is on their fire resistance properties. Many re-
ports have addressed that by using natural fibres as supplement
and/or reinforcement of thermoplastics, the amount of Carbon
Monoxide provided during fire is less than that of their host
materials.
5.2. Bio-medical applications
For biomedical applications, protein based natural fibre such as
silkworm silk, feather and spider silk fibres are suggested rather
than other type of plant based natural fibre. Silk fibres as sutures
for human wound dressing have been used for centuries [76]. Re-
cently, regenerated silk solutions have been used to form a variety
of biomaterials, such as gels, sponges and films, for medical applica-
tions [77]. Moreover, silk has been exploited as a scaffold biomate-
rial for cell culture and tissue engineering in vitro and in vivo [78].
Bioengineering is usually defined as a basic research-oriented activ-
ity closely related to biotechnology and genetic engineering which
are used for the modification of animal or plant cells, or parts of
cells, to restore their function or repair their damage regions, or
to develop new microorganisms for beneficial ends [1]. Concerning
the implementation of technology in bio-engineering, biomaterials
are mainly used in the applications of directing, supplementing, or
replacing the functions of living tissues in the human body [72].
Natural fibre composites, mainly on the animal-based fibres are
being used for bone repairs and implant development recently as a
replacement for traditional metallic materials such as stainless
steel and titanium. Although stainless steel and titanium provide
sufficient strength and rigidity to align the bone and control mo-
tion while healing of bone fracture, they are too stiff as compared
with the properties of nature bone [Alan Paper]. By using the ani-
mal based fibre as reinforcement for biodegradable polymer for
tail-making a new class of biocomposites can enhance the strength
of recovered bones and also minimise the risk of the second
surgery for removing any metallic implants inside the body. In gen-
eral, several critical issues are guided on choosing the appropriate
natural fibre composites for biomedical and bioengineering appli-
cations, these include: (1) biodegradability, (2) bioresorbability,
(3) biocompatibility, (4) sterilizability (5) functionability (6) manu-
facturability, and (7) mechanical and thermal properties [79–81].
Although many works have been conducted along the similar line
on applying animal fibres into new class of bio-grade polymer
composites, the path is still a long way to go for viva and in vivo
examinations.
6. Conclusion
The development of natural fibre reinforced polymer compos-
ites has been a hot topic recently due to the increasing environ-
mental awareness on reducing the use of fossil fuel and its
related products. Natural fibre can be classified for plant-based
and animal-based. The selection criteria are highly dependent on
their type, application and cost. However, there is still uncertain
on which type of manufacturing processes that are suitable for pro-
ducing these composites as their materials and mechanical charac-
teristics are different as compared with traditional carbon and
glass fibre composites in general. Some processes, their original de-
sign were not targeted for natural fibres, while their technologies
have been well developed for fast and reliable composite produc-
tion. This paper addresses a comprehensive review on different
3561
types of composites manufacturing process and their effects to
the natural fibre and its composites.
Acknowledgement
This project is supported by the Hong Kong Polytechnic Univer-
sity Grant (G-U688) and the University of Southern Queensland.
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